Abstract
Porous fillers have been incorporated into precursor membranes to fabricate carbon molecular sieve (CMS) membranes, where the interfacial compatibility between fillers and matrix significantly influences the separation performance of converted CMS membranes. To address this issue, we introduce molecular fillers of porous organic cages (POCs) into precursor membranes, the organic composition and discrete molecular characteristics of which can enhance the compatibility with the polymer matrix (PIM-1), bringing enhanced porosity and narrowed pore size distribution, especially in the ultra-micropore region, to the CMS membranes. The obtained CMS membrane shows simultaneously improved gas permeability and selectivity wherein the optimized CMS membrane pyrolyzed at 600 °C with 10 wt% POCs loading (CMS-10%-600) exhibits a CO2 permeability of 2002 Barrer and a CO2/CH4 selectivity of 221.6, surpassing the 2019 CO2/CH4 upper bound and superior to most of reported CMS membranes. Due to the incorporation of POC, the CMS-10%-600 membrane demonstrates a 147.5 % increase in CO2 permeability and a 297.1 % increase in CO2/CH4 selectivity compared to pristine PIM-1-based CMS membrane, along with the excellent aging resistance for over 30 days. This study provides new insights into the design of high-performance CMS membranes for gas separation.
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